A promising strategy to tailor the magnetic and electronic properties of 2D van der Waals magnets is to integrate them with a ferroelectric (FE) substrate. Herein, the FE substrate effect of BiFeO3(0001) with different surface terminations is explored using density functional theory calculations for the ferromagnetic 2H-VS2 monolayer. It is observed that depending on the polarization direction and surface termination of the BiFeO3(0001) FE substrate, the 2H-VS2/BiFeO3(0001) interface exhibits a substantially varied charge transfer behavior. The magnetic and electronic properties of the monolayer 2H-VS2 are significantly modulated by the interface charge transfer. Furthermore, in the 2H-VS2/BiFeO3(0001) heterostructures, large interface magnetoelectric coupling coefficients are predicted. The in-plane magnetic and electronic properties of monolayer 2H-VS2 can be effectively tuned by the out-of-plane FE polarization, paving the way for a novel class of spintronic devices based on the 2H-VS2/BiFeO3(0001) hybrid system.